Key Laboratory of Textile Science & Technology, Ministry of Education, College of Textiles, Donghua University, Shanghai, 201620, China.
Department of Materials Science and Engineering, National University of Singapore, Singapore, 117574, Singapore.
Small. 2023 Apr;19(15):e2206823. doi: 10.1002/smll.202206823. Epub 2023 Jan 11.
The emerging transition metal-nitrogen-carbon (MNC) materials are considered as a promising oxygen reduction reaction (ORR) catalyst system to substitute expensive Pt/C catalysts due to their high surface area and potential high catalytic activity. However, MNC catalysts are easy to be attacked by the ORR byproducts that easily lead to the deactivation of metal active sites. Moreover, a high metal loading affects the mass transfer and stability, but a low loading delivers inferior catalytic activity. Here, a new strategy of designing ZrO quantum dots and N-complex as dual chemical ligands in N-doped bubble-like porous carbon nanofibers (N-BPCNFs) to stabilize copper (Cu) by forming CuZrO /ZrO heterostructures and CuN ligands with a high loading of 40.5 wt.% is reported. While the highly porous architecture design of N-BPCNFs builds a large solidelectrolytegas phase interface and promotes mass transfer. The preliminary results show that the half-wave potential of the catalyst reaches 0.856 V, and only decreases 0.026 V after 10 000 cycles, exhibiting excellent stability. The proposed strategy of stabilizing metal active sites with both heterostructures and CuN ligands is feasible and scalable for developing high metal loading ORR catalyst.
新兴的过渡金属-氮-碳(MNC)材料由于其高比表面积和潜在的高催化活性,被认为是一种很有前途的氧还原反应(ORR)催化剂体系,可以替代昂贵的 Pt/C 催化剂。然而,MNC 催化剂很容易受到 ORR 副产物的攻击,这很容易导致金属活性位点失活。此外,高金属负载会影响传质和稳定性,但低负载会导致催化活性降低。在这里,我们报道了一种新的策略,即设计 ZrO 量子点和 N-复合物作为双化学配体,用于稳定氮掺杂泡状多孔碳纳米纤维(N-BPCNFs)中的铜(Cu),形成 CuZrO /ZrO 异质结构和 CuN 配体,Cu 的负载量高达 40.5wt.%。同时,N-BPCNFs 的高度多孔结构设计构建了大的固-液-气相间界面,促进了传质。初步结果表明,催化剂的半波电位达到 0.856V,经过 10000 次循环后仅下降 0.026V,表现出优异的稳定性。用异质结构和 CuN 配体稳定金属活性位点的这种策略对于开发高金属负载 ORR 催化剂是可行和可扩展的。